Please use this identifier to cite or link to this item: http://hdl.handle.net/2445/113212
Title: Electronic structure of stoichiometric and reduced ZnO from periodic relativistic all electron hybrid density functional calculations using numeric atom-centered orbitals
Author: Viñes Solana, Francesc
Illas i Riera, Francesc
Keywords: Teoria del funcional de densitat
Density functionals
Issue Date: 11-Jan-2017
Publisher: Wiley
Abstract: The atomic and electronic structure of stoichiometric and reduced ZnO wurtzite has been studied using a periodic relativistic all electron hybrid density functional (PBE0) approach and numeric atom-centered orbital basis set with quality equivalent to aug-cc-pVDZ. To assess the importance of relativistic effects, calculations were carried out without and with explicit inclusion of relativistic effects through the zero order regular approximation. The calculated band gap is ∼0.2 eV smaller than experiment, close to previous PBE0 results including relativistic calculation through the pseudopotential and ∼0.25 eV smaller than equivalent nonrelativistic all electron PBE0 calculations indicating possible sources of error in nonrelativistic all electron density functional calculations for systems containing elements with relatively high atomic number. The oxygen vacancy formation energy converges rather fast with the supercell size, the predicted value agrees with previously hybrid density functional calculations and analysis of the electronic structure evidences the presence of localized electrons at the vacancy site with a concomitant well localized peak in the density of states ∼0.5 eV above the top of the valence band and a significant relaxation of the Zn atoms near to the oxygen vacancy. Finally, present work shows that accurate results can be obtained in systems involving large supercells containing up to ∼450 atoms using a numeric atomic-centered orbital basis set within a full all electron description including scalar relativistic effects at an affordable cost.
Note: Versió postprint del document publicat a: https://doi.org/10.1002/jcc.24705
It is part of: Journal of Computational Chemistry, 2017, vol. 38, num. 8, p. 523-529
URI: http://hdl.handle.net/2445/113212
ISSN: 0192-8651
Appears in Collections:Publicacions de projectes de recerca finançats per la UE
Articles publicats en revistes (Ciència dels Materials i Química Física)

Files in This Item:
File Description SizeFormat 
672672.pdf2.8 MBAdobe PDFView/Open    Request a copy


Embargat   Document embargat fins el 11-1-2018


Items in DSpace are protected by copyright, with all rights reserved, unless otherwise indicated.